摘要
合成了Co/Al双金属氧化物催化剂,并将其用于催化还原糠醛制备糠醇。通过调节Co/Al的物质的量之比,探讨了活性金属的比例对催化剂物理、化学性质的影响。N_(2)吸附/脱附等温线分析表明,制备得到的系列Co_(x)AlO_(y)催化剂为平均孔径20 nm左右的介孔材料;NH_(3)-TPD分析表明,中等强度酸位点占主导有利于糠醛加氢制糠醇。Co/Al物质的量比3∶1时制得的催化剂Co_(3)AlO_(x)表现出优异的催化活性,在反应物0.3 g糠醛、溶剂20 mL 1,4-二氧六环、催化剂Co_(3)AlO_(x)用量0.12 g,反应时间3 h,H_(2)压力2 MPa,反应温度120℃条件下,糠醛转化率超过98.95%,糠醇得率可以达到96.25%。XRD、TEM和XPS分析表明:Co_(3)AlO_(x)以CoAl_(2)O_(4)和Co_(2)O_(3)的混合相形式存在,比表面积和中等强度酸是影响催化活性的关键因素。Co_(3)AlO_(x)催化剂经过5次循环实验后,催化活性仍能保持83.13%,具有十分良好的循环稳定性。
Co/Al bimetallic oxide catalyst was prepared and used for catalytic reduction of furfural to furfuryl alcohol.The effects of the active metal ratio on the physical and chemical properties of the catalyst were discussed by adjusting the molar ratio of Co/Al.N_(2) adsorption/desorption analysis showed that the series of prepared Co_(x)AlO_(y) catalysts were mesoporous materials with an average pore size of about 20 nm.NH_(3)-TPD analysis showed that the dominance of moderate acid sites was favorable for hydrogenation of furfural to furfuryl alcohol.The prepared Co_(3)AlO_(x) with the Co/Al molar ratio of 3∶1 exhibited excellent catalytic activity.Under the operational conditions of 0.3 g furfuryl alcohol,20 mL solvent 1,4-dioxane,0.12 g catalyst Co_(3)AlO_(x),reaction time 3 h,H_(2) pressure 2 MPa and reaction temperature 120℃,the conversion of furfuryl alcohol was more than 98.95%,and the yield of furfuryl alcohol could reach 96.25%.XRD,TEM and XPS analysis showed that Co_(3)AlO_(x) existed in the mixed phase of CoAl_(2)O_(4) and Co_(2)O_(3),and the specific surface area and moderate acid strength were the key factors determining the catalytic activity.The catalytic activity of Co_(3)AlO_(x) catalyst could still maintain 83%after 5 cycles,which indicates its good cycle stability.
作者
姜伟
辛颖
巩明月
王伟众
王东军
孙勇
JIANG Wei;XIN Ying;GONG Mingyue;WANG Weizhong;WANG Dongjun;SUN Yong(China Petroleum Petrochemical Research Institute Daqing Petrochemical Research Center,Daqing 163714,China;College of Energy,Xiamen University,Fujian Engineering and Research Center of Clean and High-valued Technologies for Biomass,Xiamen Key Laboratory of Clean and High-valued Utilization for Biomass,Xiamen 361102,China)
出处
《林产化学与工业》
CAS
CSCD
北大核心
2022年第5期8-14,共7页
Chemistry and Industry of Forest Products
基金
国家自然科学基金资助项目(21776234)。
关键词
糠醛
糠醇
催化还原
钴铝双金属氧化物
furfural
furfuryl alcohol
catalytic reduction
Co/Al bimetallic oxide